Three-Motif Molecular Junction Type Covalent Organic Frameworks for Efficient Photocatalytic Aerobic Oxidation

• DOI: 10.1021/jacs.3c12724
• Publication Date: 2024-01-24T23:11:10Z
• Authors: Ming-Yi Yang; Shuai-Bing Zhang; Mi Zhang; Ze-Hui Li; Yu-Fei Liu; Xing Liao; Meng Lu; Shun-Li Li; Ya-Qian Lan
• Keywords: Benzylamine; Triphenylamine

Covalent organic frameworks (COFs), with the features of flexible structure regulation and easy introduction functional groups, have aroused broad interest in field photocatalysis. However, due to low light absorption intensity, photoelectron conversion efficiency, lack suitable active sites, it remains a great challenge achieve efficient photocatalytic aerobic oxidation reactions. Herein, based on reticular chemistry, we rationally designed series three-motif molecular junction type COFs, which formed dual photosensitizer coupled redox junctions containing multifunctional COF photocatalysts. Significantly, strong adsorption ability units integrated reduction features, PY-BT exhibited highest activity for oxidation. Especially, achieved benzylamine efficiency 99.9% 2.5 h, is much higher than that two-motif only one or unit lacking COFs. The mechanism selective was studied through comprehensive experiments density theory calculations. results showed photoinduced electron transfer occurred from PY then triphenylamine BT. Furthermore, thermodynamics energy lower others, confirmed synergistic effect This work provided new strategy design COFs also represented insight into catalytic